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Biporous Metal-Organic Framework with Tunable CO₂/CH₄ Separation Performance Facilitated by Intrinsic Flexibility.

ABSTRACT: In this work, we report the synthesis of SION-8, a novel metal-organic framework (MOF) based on Ca(II) and a tetracarboxylate ligand TBAPy^4- endowed with two chemically distinct types of pores characterized by their hydrophobic and hydrophilic properties. By altering the activation conditions, we gained access to two bulk materials: the fully activated SION-8F and the partially activated SION-8P with exclusively the hydrophobic pores activated. SION-8P shows high affinity for both CO₂ ( Q_st = 28.4 kJ/mol) and CH₄ ( Q_st = 21.4 kJ/mol), while upon full activation, the difference in affinity for CO₂ ( Q_st = 23.4 kJ/mol) and CH₄ ( Q_st = 16.0 kJ/mol) is more pronounced. The intrinsic flexibility of both materials results in complex adsorption behavior and greater adsorption of gas molecules than if the materials were rigid. Their CO₂/CH₄ separation performance was tested in fixed-bed breakthrough experiments using binary gas mixtures of different compositions and rationalized in terms of molecular interactions. SION-8F showed a 40-160% increase (depending on the temperature and the gas mixture composition probed) of the CO₂/CH₄ dynamic breakthrough selectivity compared to SION-8P, demonstrating the possibility to rationally tune the separation performance of a single MOF by manipulating the stepwise activation made possible by the MOF's biporous nature.

SUBMITTER: Gladysiak A

PROVIDER: S-EPMC6202632 | biostudies-literature | 2018 Oct

REPOSITORIES: biostudies-literature

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Biporous Metal-Organic Framework with Tunable CO2/CH4 Separation Performance Facilitated by Intrinsic Flexibility.

Gładysiak Andrzej A Deeg Kathryn S KS Dovgaliuk Iurii I Chidambaram Arunraj A Ordiz Kaili K Boyd Peter G PG Moosavi Seyed Mohamad SM Ongari Daniele D Navarro Jorge A R JAR Smit Berend B Stylianou Kyriakos C KC

ACS applied materials & interfaces 20181011 42

In this work, we report the synthesis of SION-8, a novel metal-organic framework (MOF) based on Ca(II) and a tetracarboxylate ligand TBAPy4- endowed with two chemically distinct types of pores characterized by their hydrophobic and hydrophilic properties. By altering the activation conditions, we gained access to two bulk materials: the fully activated SION-8F and the partially activated SION-8P with exclusively the hydrophobic pores activated. SION-8P shows high affinity for both CO< ...[more]

PMID: 30247880

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Project description:Global warming is arguably the biggest scientific challenge of the twenty-first century and its environmental consequences are already noticeable. To mitigate the emissions of greenhouse gases, particularly of CO2, there is an urgent need to design materials with improved adsorbent properties. Five different magnetic ionic liquids were impregnated into the metal-organic framework ZIF-8. The composites were produced by a direct-contact method, and their performance as sorbents for gas separation applications was studied. The impact of the ionic liquid anion on the sorption capacity and ideal CO2/CH4 and CO2/N2 selectivities were studied, focusing on understanding the influence of metal atom and ligand on the adsorbent properties. Reproducible methodology, along with rigorous characterization, were established to assess the impact of the ionic liquid on the performance of the composite materials. Results show that the ionic liquid was well-impregnated, and the ZIF-8 structure was maintained after ionic liquid impregnation. The produced composites were of microporous nature and were thermally stable. CO2, CH4, and N2 adsorption-desorption isotherms were obtained at 303 K and between 0 and 16 bar. The adsorption-desorption data of the composites were compared with that obtained for original ZIF-8. The general trend in composites is that the increased gas uptake per available pore volume compensates the pore volume loss. Adsorption data per unit mass showed that composites have reversible sorption, but inferior gas uptake at all pressure ranges. This is due to the observed total pore volume loss by the ionic liquid pore occupation/blockage. In most cases, composites showed superior selectivity performance at all pressure range. In particular, the composite [C4MIM]2[MnCl4]@ZIF-8 shows a different low-pressure selectivity trend from the original MOF, with a 33% increase in the CO2/N2 selectivity at 1 bar and 19% increase in the CO2/CH4 selectivity at 10 bar. This material shows potential for use in a post-combustion CO2 capture application that can contribute to greenhouse gas mitigation.

Dataset Information

Biporous Metal-Organic Framework with Tunable CO₂/CH₄ Separation Performance Facilitated by Intrinsic Flexibility.

Publications

Biporous Metal-Organic Framework with Tunable CO<sub>2</sub>/CH<sub>4</sub> Separation Performance Facilitated by Intrinsic Flexibility.

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